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Applied Physics Letters

Single-domain spectroscopy of self-assembled photonic crystals

Yu. A. Vlasov, Miriam Deutsch, David J. Norris

Published Mar 20, 2000• 127 citations
Publisher

Abstract

We show how optical microscopy can be used to study the optical properties of a single crystalline domain in a self-assembled photonic crystal. By measuring spatially resolved reflection and emission spectra from a synthetic opal, inhomogeneities due to averaging over inherent disorder can be avoided. From “defect-free” reflection and emission spectra, the intrinsic photonic band structure can be extracted and inhibition of spontaneous emission can be verified.

DOI
10.1063/1.126117

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We show how optical microscopy can be used to study the optical properties of a single crystalline domain in a self-assembled photonic crystal. By measuring spatially resolved reflection and emission spectra from a synthetic opal, inhomogeneities due to averaging over inherent disorder can be avoided. From “defect-free” reflection and emission spectra, the intrinsic photonic band structure can be extracted and inhibition of spontaneous emission can be verified.
We have performed angle-resolved measurements of spontaneous-emission spectra from laser dyes and quantum dots in opal and inverse opal photonic crystals. Pronounced directional dependencies of the emission spectra are observed: angular ranges of strongly reduced emission adjoin with angular ranges of enhanced emission. It appears that emission from embedded light sources is affected both by the periodicity and by the structural imperfections of the crystals: the photons are Bragg diffracted by lattice planes and scattered by unavoidable structural disorder. Using a model comprising diffuse light transport and photonic band structure, we quantitatively explain the directional emission spectra. This work provides detailed understanding of the transport of spontaneously emitted light in real photonic crystals, which is essential in the interpretation of quantum optics in photonic-band-gap crystals and for applications wherein directional emission and total emission power are controlled.
We present the application of spectral emission imaging microscopy as a method to quantitatively map photonic properties from below the surface of strongly interacting photonic three-dimensional (3D) crystals. We excite emission from emitters deep inside a photonic crystal and record the local emission spectra with micrometer lateral resolution. The recorded directional emission spectra are modified by Bragg diffraction, which we use to determine the local stop-band attenuation, center frequency, and width. Assembling the values obtained into spatial maps yields detailed access to the distributions of the local photonic properties below the crystal surface. We demonstrate this approach by analyzing the emission from the fluorescent protein DsRed2 infiltrated inside self-organized 3D titanium dioxide inverse opals.
We present the first experiments that demonstrate strong angle-independent modification of spontaneous emission spectra from laser dyes in photonic crystals, made of inverse opals in titania. We show that both the fluorescence quantum efficiency and weak disorder play a key role in interpreting the experimental data. We compare the angle-independent emission spectra of dye in photonic crystals with spectra from such crystals with much smaller lattice spacings, for which emission is in the long wavelength limit. The ratio of emission power spectra shows inhibition of emission up to a factor ∼ 5 over a large bandwidth of 13% of the first order Bragg resonance frequency. The inhibition shifts to increasing wavelength with the lattice parameter, confirming the photonic nature of the phenomenon. The center frequency and bandwidth of the inhibition agree with the calculated total density of states, but the measured inhibition of the vacuum fluctuations is much larger. This result is confirmed by experiments using different dyes. We likely probe the strongly modulated local photonic density of states, due to the spatially nonuniform distribution of dye molecules over the unit cell.
The propagation and emission of light in a real photonic crystal is routinely affected by the intrinsic disorder and its finite-size. Thus, theoretical calculation based on the notion of a defect free crystal with an infinite thickness is irrational in the real world experiments. Here, we report an acute modification of light propagation and emission induced by the finite-size of the crystal. We have measured the emission intensity and rate from single domain of the crystal to study the finite size effect on the spontaneous emission suppression. The results show spatial fluctuation of spontaneous emission suppression across domains that have a linear scaling with crystal size. The results have implications in contriving devices pertaining to controlled spontaneous emission such as in cavity quantum electrodynamics.
The photonic dispersion, the group-velocity dispersion, the effective mass, refractive index, and the spectral distribution of the density of photonic states near the edge of the photonic stop band are numerically calculated in the one-dimensional model for photonic crystals based on synthetic opals. The fluorescence spectra of rhodamine 6G and 2,5-bis(2-benzoxazolyl)hydroquinone molecules infiltrated into a synthetic opal are measured. For both substances, it is observed that the spontaneous emission intensity in the range of the photonic stop band is appreciably suppressed. A blue shift of the fluorescence spectrum of rhodamine 6G molecules is revealed. Secondary emission of synthetic opals infiltrated with colloidal silver is observed in the Stokes range under excitation of opals by radiation at λ = 400 nm. The spectrum of the secondary emission is located in the range 450–590 nm, which contains the stop band and intervals near its edges.